No Arabic abstract
Noise-immune cavity-enhanced optical frequency comb spectroscopy (NICE-OFCS) is a recently developed technique that utilizes phase modulation to obtain immunity to frequency-to-amplitude noise conversion by the cavity modes and yields high absorption sensitivity over a broad spectral range. We describe the principles of the technique and discuss possible comb-cavity matching solutions. We present a theoretical description of NICE-OFCS signals detected with a Fourier transform spectrometer (FTS), and validate the model by comparing it to experimental CO2 spectra around 1575 nm. Our system is based on an Er:fiber femtosecond laser locked to a cavity and phase-modulated at a frequency equal to a multiple of the cavity free spectral range (FSR). The NICE-OFCS signal is detected by a fast-scanning FTS equipped with a high-bandwidth commercial detector. We demonstrate a simple method of passive locking of the modulation frequency to the cavity FSR that significantly improves the long term stability of the system, allowing averaging times on the order of minutes. Using a cavity with a finesse of ~9000 we obtain absorption sensitivity of 6.4 x 10^{-11} cm^{-1} Hz^{-1/2} per spectral element, and concentration detection limit for CO2 of 450 ppb Hz^{-1/2}, determined by multiline fitting.
We present broadband cavity-enhanced complex refractive index spectroscopy (CE-CRIS), a technique for calibration-free determination of the complex refractive index of entire molecular bands via direct measurement of transmission modes of a Fabry-Perot cavity filled with the sample. The measurement of the cavity transmission spectrum is done using an optical frequency comb and a mechanical Fourier transform spectrometer with sub-nominal resolution. Molecular absorption and dispersion spectra (corresponding to the imaginary and real parts of the refractive index) are obtained from the cavity mode broadening and shift retrieved from fits of Lorentzian profiles to the individual cavity modes. This method is calibration-free because the mode broadening and shift are independent of the cavity parameters such as the length and mirror reflectivity. In this first demonstration of broadband CE-CRIS we measure simultaneously the absorption and dispersion spectra of three combination bands of CO2 in the range between 1525 nm and 1620 nm and achieve good agreement with theoretical models. This opens up for precision spectroscopy of the complex refractive index of several molecular bands simultaneously.
Broadband ultrafast optical spectroscopy methods, such as transient absorption spectroscopy and 2D spectroscopy, are widely used to study molecular dynamics. However, these techniques are typically restricted to optically thick samples, such as solids and liquid solutions. In this article we discuss a cavity-enhanced ultrafast transient absorption spectrometer covering almost the entire visible range with a detection limit of $Delta$OD $ < 1 times 10^{-9}$, extending broadband all-optical ultrafast spectroscopy techniques to dilute beams of gas-phase molecules and clusters. We describe the technical innovations behind the spectrometer and present transient absorption data on two archetypical molecular systems for excited-state intramolecular proton transfer, 1-hydroxy-2-acetonapthone and salicylideneaniline, under jet-cooled and Ar cluster conditions.
We demonstrate optical frequency comb Faraday rotation spectroscopy (OFC-FRS) for broadband interference-free detection of paramagnetic species. The system is based on a femtosecond doubly resonant optical parametric oscillator and a fast-scanning Fourier transform spectrometer (FTS). The sample is placed in a DC magnetic field parallel to the light propagation. Efficient background suppression is implemented via switching the direction of the field on consecutive FTS scans and subtracting the consecutive spectra, which enables long term averaging. In this first demonstration, we measure the entire Q- and R-branches of the fundamental band of nitric oxide in the 5.2-5.4 {mu}m range and achieve good agreement with a theoretical model.
Optomechanical devices operated at their quantum limit open novel perspectives for the ultrasensitive determination of mass and displacement, and also in the broader field of quantum technologies. The access to higher frequencies implies operation at higher temperatures and stronger immunity to environmental noise. We propose and demonstrate here a new concept of quantum well photoelastic comb for the efficient coupling of light to optomechanical resonances at hundreds of GHz in semiconductor hybrid resonators. A purposely designed ultra-high resolution Raman spectroscopy set-up is exploited to evidence the transfer of spectral weight from the mode at 60 GHz to modes at 190-230 GHz, corresponding to the $8^{th}$ and $10^{th}$ overtone of the fundamental breathing mode of the light-sound cavities. The coupling to mechanical frequencies two orders of magnitude larger than alternative approaches is attained without reduction of the optomechanical constant $g_0$. The wavelength dependence of the optomechanical coupling further proves the role of resonant photoelastic interaction, highlighting the potentiality to access strong-coupling regimes. The experimental results show that electrostrictive forces allow for the design of devices optimized to selectively couple to specific mechanical modes. Our proposal opens up exciting opportunities towards the implementation of novel approaches applicable in quantum and ultra-high frequency information technologies.
Spectroscopy in the molecular fingerprint spectral region (6.5-20 $mu$m) yields critical information on material structure for physical, chemical and biological sciences. Despite decades of interest and effort, this portion of the electromagnetic spectrum remains challenging to cover with conventional laser technologies. In this report, we present a simple and robust method for generating super-octave, optical frequency combs in the fingerprint region through intra-pulse difference frequency generation in an orientation-patterned gallium phosphide crystal. We demonstrate the utility of this unique coherent light source for high-precision, dual-comb spectroscopy in methanol and ethanol vapor. These results highlight the potential of laser frequency combs for a wide range of molecular sensing applications, from basic molecular spectroscopy to nanoscopic imaging.